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A novel channel-wall engineering strategy of the porous materials cationic covalent organic frameworks (COFs) is established based on rapid microwave-assisted anion exchange reaction and utilized to prepare a set of new COFs. Due to the interaction between the carbon dioxide (CO2) and the acetate anion, the resulting SJTU-COF-AcO shows greatly enhanced carbon dioxide capacity up to 1.7 times of the pristine COF. The effect of the counter anions to CO2 capacity in the cationic COFs is investigated for the first time, which demonstrates that our channel-wall engineering strategy is a promising way to tailor the property of COFs for high CO2 capacity.